Influence of the Sintering Temperature on LLZO-NCM Cathode Composites for Solid-State Batteries Studied by Transmission Electron Microscopy

Demuth, Thomas P.; Fuchs, Till; Rohnke, Marcus; Pokle, Anuj; Ahmed, Shamail; Malaki, Michael; Beyer, Andreas; Janek, Jürgen; Volz, Kerstin

doi:10.2139/ssrn.4323721

Cited by 2 publications

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“…Given that the interphase gradually changes from Li-ion conductor to Li-deficient species with lower conductivity, the increment of interfacial impedance is attributed to the interfacial structure transition. [62,63] Mechanistic insights into thermal-induced interfacial evolution are proposed in Figure 6, showing the interplay of SCL, chemical potential of Mn (μ Mn ), Mn ion distribution (C Mn ), and interphase transition. At RT, SCL naturally forms at the boundary between cathode and SSE, which is mainly due to the rebalance of interfacial chemical potential and consequent charge carrier redistribution.…”

Section: Resultsmentioning

confidence: 99%

Thermal‐Induced Structure Evolution at the Interface between Cathode and Solid‐State Electrolyte

Lei,

Wang,

et al. 2023

Small Structures

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The interfaces between the electrode and solid‐state electrolyte play a decisive role in the performance of all‐solid‐state batteries. For example, the formation of the interphase between cathode and solid‐state electrolyte can affect interfacial impedance and thus the rate capability. Herein, the thermal stability at the solid–solid interface between LiMn2O4 cathode and garnet electrolyte LLZTO via combined in situ techniques is studied, including in situ X‐Ray diffraction, in situ transmission electron microscopy, and in situ Raman. The dynamic process of interfacial reaction at different scales is elucidated. Starting from 300 °C, Mn ions from LiMn2O4 would migrate into the solid‐state electrolyte, accompanied with the formation of LiMn3O4 interphase. As the temperature increases to 500 °C, the LiMn3O4 interphase transforms to MnO structure which hinders Li‐ion transportation and therefore increases the interfacial impedance. Although both LiMn2O4 and LLZTO could withstand continuous heating, their interface is inherently thermally unstable at relatively low temperature, which requires special attention during thermal treatment for practical fabrication. Findings provide mechanistic insights into the interfacial reaction which serves as a guidance for the design and manufacturing of all‐solid‐state batteries.

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Section: Resultsmentioning

confidence: 99%

Thermal‐Induced Structure Evolution at the Interface between Cathode and Solid‐State Electrolyte

Lei,

Wang,

et al. 2023

Small Structures

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“…[49] Accordingly, they are inapplicable for dealing with Li 2 CO 3 at Ni-rich cathode/LLZTO and Li/LLZTO interfaces because LaNiO 3 species are formed at 500 °C and Li melts at ≈180°C. [50] Therefore, it is quite necessary to handle Li 2 CO 3 at all interfaces among cathode, electrolyte and anode to fundamentally decrease interface resistances and enable highvoltage SSLBs.…”

Section: Introductionmentioning

confidence: 99%

Fluorinating All Interfaces Enables Super‐Stable Solid‐State Lithium Batteries by In Situ Conversion of Detrimental Surface Li₂CO₃

Guo,

Pan,

et al. 2023

Advanced Materials

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Li‐stuffed battery materials intrinsically have surface impurities, typically Li2CO3, which introduce severe kinetic barriers and electrochemical decay for a cycling battery. For energy‐dense solid‐state lithium batteries (SSLBs), mitigating detrimental Li2CO3 from both cathode and electrolyte materials is required, while the direct removal approaches hardly avoid Li2CO3 regeneration. Here, a decarbonization–fluorination strategy to construct ultrastable LiF‐rich interphases throughout the SSLBs by in situ reacting Li2CO3 with LiPF6 at 60 °C is reported. The fluorination of all interfaces effectively suppresses parasitic reactions while substantially reducing the interface resistance, producing a dendrite‐free Li anode with an impressive cycling stability of up to 7000 h. Particularly, transition metal dissolution associated with gas evolution in the cathodes is remarkably reduced, leading to notable improvements in battery rate capability and cyclability at a high voltage of 4.5 V. This all‐in‐one approach propels the development of SSLBs by overcoming the limitations associated with surface impurities and interfacial challenges.

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Influence of the Sintering Temperature on LLZO-NCM Cathode Composites for Solid-State Batteries Studied by Transmission Electron Microscopy

Cited by 2 publications

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Thermal‐Induced Structure Evolution at the Interface between Cathode and Solid‐State Electrolyte

Thermal‐Induced Structure Evolution at the Interface between Cathode and Solid‐State Electrolyte

Fluorinating All Interfaces Enables Super‐Stable Solid‐State Lithium Batteries by In Situ Conversion of Detrimental Surface Li₂CO₃

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Influence of the Sintering Temperature on LLZO-NCM Cathode Composites for Solid-State Batteries Studied by Transmission Electron Microscopy

Cited by 2 publications

References 0 publications

Thermal‐Induced Structure Evolution at the Interface between Cathode and Solid‐State Electrolyte

Thermal‐Induced Structure Evolution at the Interface between Cathode and Solid‐State Electrolyte

Fluorinating All Interfaces Enables Super‐Stable Solid‐State Lithium Batteries by In Situ Conversion of Detrimental Surface Li2CO3

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Product

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Fluorinating All Interfaces Enables Super‐Stable Solid‐State Lithium Batteries by In Situ Conversion of Detrimental Surface Li₂CO₃